Highly Efficient Electrocatalytic Oxygen Evolution Over Atomically Dispersed Synergistic Ni/Co Dual Sites

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(40)

Published: July 27, 2022

Single-atom catalysts (SACs) are being pursued as economical electrocatalysts. However, their low active-site loading, poor interactions, and unclear catalytic mechanism call for significant advances. Herein, atomically dispersed Ni/Co dual sites anchored on nitrogen-doped carbon (a-NiCo/NC) hollow prisms rationally designed synthesized. Benefiting from the dual-metal synergistic obtained a-NiCo/NC sample exhibits superior electrocatalytic activity kinetics towards oxygen evolution reaction. Moreover, density functional theory calculations indicate that strong interactions heteronuclear paired lead to optimization of electronic structure reduced reaction energy barrier. This work provides a promising strategy synthesis high-efficiency dual-site SACs in field electrochemical storage conversion.

Language: Английский

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Interfacial assembly of binary atomic metal-Nx sites for high-performance energy devices

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: April 1, 2023

Abstract Anion-exchange membrane fuel cells and Zn–air batteries based on non-Pt group metal catalysts typically suffer from sluggish cathodic oxygen reduction. Designing advanced catalyst architectures to improve the catalyst’s reduction activity boosting accessible site density by increasing loading utilization are potential ways achieve high device performances. Herein, we report an interfacial assembly strategy binary single-atomic Fe/Co-N x with mass loadings through constructing a nanocage structure concentrating high-density Fe/Co–N sites in porous shell. The prepared FeCo-NCH features distribution as 7.9 wt% of around 7.6 × 10 19 g −1 , surpassing most reported M–N catalysts. In anion exchange zinc–air batteries, material delivers peak power densities 569.0 or 414.5 mW cm −2 3.4 2.8 times higher than control devices assembled FeCo-NC. These results suggest that present for promoting catalytic offers new possibilities exploring efficient low-cost electrocatalysts boost performance various energy devices.

Language: Английский

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Geminal-atom catalysis for cross-coupling

Nature, Journal Year: 2023, Volume and Issue: 622(7984), P. 754 - 760

Published: Sept. 20, 2023

Language: Английский

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Regulating the scaling relationship for high catalytic kinetics and selectivity of the oxygen reduction reaction

Nature Communications, Journal Year: 2022, Volume and Issue: 13(1)

Published: Oct. 27, 2022

The electrochemical oxygen reduction reaction (ORR) is at the heart of modern sustainable energy technologies. However, linear scaling relationship this multistep now becomes bottleneck for accelerating kinetics. Herein, we propose a strategy using intermetallic-distance-regulated atomic-scale bimetal assembly (ABA) that can catalyse direct O‒O radical breakage without formation redundant *OOH intermediates, which could regulate inherent and cause ORR on ABA to follow fast-kinetic dual-sites mechanism. Using in situ synchrotron spectroscopy, directly observe self-adjustable N-bridged Pt = N2 Fe promotes generation key intermediate state (Pt‒O‒O‒Fe) during process, resulting high kinetics selectivity. well-designed catalyst achieves nearly two orders magnitude enhanced kinetic current density half-wave potential 0.95 V relative commercial Pt/C an almost 99% efficiency 4-electron pathway selectivity, making it one catalysts application device zinc‒air cells. This study provides helpful design principle developing optimizing other efficient electrocatalysts.

Language: Английский

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Asymmetric CoN₃P₁ Trifunctional Catalyst with Tailored Electronic Structures Enabling Boosted Activities and Corrosion Resistance in an Uninterrupted Seawater Splitting System

Advanced Materials, Journal Year: 2022, Volume and Issue: 34(34)

Published: July 5, 2022

Employing seawater splitting systems to generate hydrogen can be economically advantageous but still remains challenging, particularly for designing efficient and high Cl- -corrosion resistant trifunctional catalysts toward the oxygen reduction reaction (ORR), evolution (OER), (HER). Herein, single CoNC with well-defined symmetric CoN4 sites are selected as atomic platforms electronic structure tailoring. Density function theory reveals that P-doping into lead formation of asymmetric CoN3 P1 symmetry-breaking structures, enabling affinity strong oxygen-containing intermediates, moderate H adsorption, weak adsorption. Thus, ORR/OER/HER activities stability optimized simultaneously resistance. The based catalyst boosted performance endows seawater-based Zn-air batteries (S-ZABs) superior long-term over 750 h allows operate continuously 1000 h. A self-driven powered by S-ZABs gives ultrahigh H2 production rates 497 μmol h-1 . This work is first advance scientific understanding competitive adsorption mechanism between intermediates from perspective structure, paving way synthesis

Language: Английский

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Atomically Dispersed Ni–Cu Catalysts for pH‐Universal CO₂ Electroreduction

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(13)

Published: Jan. 10, 2023

CO2 electroreduction is of great significance to reduce emissions and complete the carbon cycle. However, unavoidable carbonate formation low utilization efficiency in neutral or alkaline electrolytes hinder its application at commercial scale. The development reduction under acidic conditions provides a promising strategy, but inhibition hydrogen evolution reaction difficult. Herein, first work design Ni-Cu dual atom catalyst supported on hollow nitrogen-doped reported for pH-universal CO. shows high CO Faradaic ≈99% acidic, neutral, electrolytes, partial current densities reach 190 ± 11, 225 10, 489 14 mA cm-2 , respectively. In particular, reaches 64.3%, which twice as that conditions. Detailed study indicates existence electronic interaction between Ni Cu atoms. atoms push d-band center further toward Fermi level, thereby accelerating *COOH. addition, operando characterizations density functional theory calculation are used elucidate possible mechanism electrolytes.

Language: Английский

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Tailor‐Engineered 2D Cocatalysts: Harnessing Electron–Hole Redox Center of 2D g‐C₃N₄ Photocatalysts toward Solar‐to‐Chemical Conversion and Environmental Purification

Advanced Functional Materials, Journal Year: 2022, Volume and Issue: 32(29)

Published: Feb. 23, 2022

Abstract Sparked by natural photosynthesis, solar photocatalysis using metal‐free graphitic carbon nitride (g‐C 3 N 4 ) with appealing electronic structure has turned up as the most captivating technique to quest for sustainable energy generation and pollution‐free environment. Nonetheless, low‐dimensional g‐C is thwarted from sluggish kinetics rapid recombination of photogenerated carriers upon light irradiation. Among multifarious modification strategies, engineering 2D cocatalysts anticipated accelerate redox kinetics, augment active sites ameliorate electron–hole separation boosted activity thanks its face‐to‐face contact surface. It timely technological significance review 2D/2D interfaces state‐of‐the‐art cocatalysts, spanning carbon‐containing phosphorus‐containing, metal dichalcogenide, other cocatalysts. Fundamental principles each photocatalytic application will be introduced. Thereafter, recent advances cocatalyst‐mediated systems critically evaluated based on their interfacial engineering, emerging roles, impacts toward stability catalytic efficiency. Importantly, mechanistic insights into charge dynamics structure–performance relationship deciphered. Last, noteworthy research directions are prospected deliver insightful ideas future development . Overall, this serve a scaffold cornerstone in designing dimensionality‐dependent cocatalyst‐assisted renewable ecologically green

Language: Английский

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Interface Engineering of NixSy@MnOxHy Nanorods to Efficiently Enhance Overall-Water-Splitting Activity and Stability

Nano-Micro Letters, Journal Year: 2022, Volume and Issue: 14(1)

Published: May 3, 2022

Three-dimensional (3D) core-shell heterostructured NixSy@MnOxHy nanorods grown on nickel foam (NixSy@MnOxHy/NF) were successfully fabricated via a simple hydrothermal reaction and subsequent electrodeposition process. The NixSy@MnOxHy/NF shows outstanding bifunctional activity stability for hydrogen evolution oxygen reaction, as well overall-water-splitting performance. main origins are the interface engineering of NixSy@MnOxHy, shell-protection characteristic MnOxHy, 3D open nanorod structure, which remarkably endow electrocatalyst with high stability. Exploring highly active stable transition metal-based electrocatalysts has recently attracted extensive research interests achieving inherent activity, abundant exposed sites, rapid mass transfer, strong structure overall water splitting. Herein, an coupled strategy was applied to construct three-dimensional heterostructure electrocatalyst. synthesized facile followed by X-ray absorption fine spectra reveal that Mn-S bonds connect interfaces leading electronic interaction, improves intrinsic activities (OER). Besides, efficient protective shell, MnOxHy dramatically inhibits electrochemical corrosion at current densities, enhances potentials. Furthermore, not only exposes enriched but also accelerates electrolyte diffusion bubble desorption. Therefore, exhibits exceptional splitting, low overpotentials 326 356 mV OER 100 500 mA cm-2, respectively, along 150 h cm-2. it presents cell voltage 1.529 V 10 accompanied excellent cm-2 h. This work sheds light exploring strategy.

Language: Английский

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Boosting oxygen reduction reaction with Fe and Se dual-atom sites supported by nitrogen-doped porous carbon

Applied Catalysis B Environment and Energy, Journal Year: 2022, Volume and Issue: 308, P. 121206 - 121206

Published: Feb. 11, 2022

Language: Английский

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Atomically precise electrocatalysts for oxygen reduction reaction

Chem, Journal Year: 2023, Volume and Issue: 9(2), P. 280 - 342

Published: Feb. 1, 2023

Language: Английский

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